The Mg 2 Al 4 Si 5 O 18 ceramic is considered as a kind of important candidates for millimeter-wave applications. In this work, Mg 2x Cu x Al 4 Si 5 O 18 (0 � x � 0.16) ceramics were synthesized by solidstate reaction, aiming to improve the microwave dielectric properties. According to the X-ray powder diffraction (XRD) analysis, Cu 2 + ions enter into the Mg 2 Al 4 Si 5 O 18 lattice and form a solid solution. The dense microstructure was observed in the Cu-substituted Mg 2 Al 4 Si 5 O 18 ceramics at x = 0.04 sintered at 1420°C. The dielectric constant (ɛ r ) values depend on the microstructure, secondary phase and ionic polarizability of the samples. The quality factor (Qf) values are dominated by the microstructure, secondary phase and centro-symmetry of [Si 4 Al 2 ] hexagonal ring. The temperature coefficients of resonance frequency (τ f ) are strongly related to the Mg/CuÀ O bond valance. In comparison to pure Mg 2 Al 4 Si 5 O 18 ceramics, the excellent microwave dielectric properties with ɛ r = 4.56, Qf = 31,100 GHz and τ f = À 52 ppm/°C were obtained at x = 0.04 with sintering at 1420°C. Thus, the Mg 2-x Cu x Al 4 Si 5 O 18 (0 � x � 0.16) ceramics will be promising millimeter-wave communication materials.